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Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence. | LitMetric

Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence.

Chem Mater

Optoelectronic Materials Section, Faculty of Applied Sciences, Delft University of Technology, Van der Maasweg 9, 2629 HZ Delft, The Netherlands.

Published: May 2021

Trap states play a crucial role in the design of colloidal quantum dot (QD)-based technologies. The presence of these in-gap states can either significantly limit the efficiency of devices (e.g., in solar cells or LEDs) or play a pivotal role in the functioning of the technology (e.g., in catalysis). Understanding the atomistic nature of traps is therefore of the highest importance. Although the mechanism through which undercoordinated chalcogenide atoms can lead to trap states in II-VI QDs is generally well understood, the nature of metal-based traps remains more elusive. Previous research has shown that reduction of metal sites in negatively charged QDs can lead to in-gap states. Here, we use density functional theory to show that metal-based traps are also formed in charge-neutral but photoexcited CdSe QDs. It is found that Cd-Cd dimers and the concomitant trap states are transient in nature and appear and disappear on the picosecond time scale. Subsequent nonradiative recombination from the trap is shown to be much faster than radiative recombination, indicating that dimer-related trap states can quench the photoluminescence. These results are expected to be transferable to other II-VI materials and highlight the importance of surface redox reactions for the optical properties of QDs. Moreover, they show that photoexcitation can lead to atomic rearrangements on the surface and thus create transient in-gap states.

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Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8154315PMC
http://dx.doi.org/10.1021/acs.chemmater.1c00561DOI Listing

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